As conventional organic solvents present inherent toxicity, deep eutectic solvents (DES) have been considered as excellent candidates due to their green characteristics. In this work, thermoelectric properties enhancement of PEDOT:PSS films is achieved by introducing DES as an additive and postātreatment reagent. Direct addition and postātreatment approaches lead to a maximum Seebeck coefficient of 29.1 Ī¼V Kā1 and electrical conductivity of 620.6 S cmā1, respectively. In addition, an optimal power factor is obtained by DES postātreatment, reaching up to 24.08 Ī¼W mā1 Kā2, which is approximately four orders of magnitude higher than the pure PEDOT:PSS. Assuming a thermal conductivity of 0.17 W mā1 Kā1, the maximum ZT value is estimated to be 0.042 at 300 K. Further, atomic force microscopy and Xāray photoelectron spectroscopy are performed and suggest that the remarkably enhanced electrical conductivity originates from the removal of the excess insulating PSS and the phase separation between the PEDOT and PSS chains. Ā© 2015 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2015, 53, 885ā892